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Carbas 

et al. Appl Adhes Sci (2021) 9:1


https://doi.org/10.1186/s40563-020-00132-5

RESEARCH Open Access

The influence of epoxy adhesive toughness


on the strength of hybrid laminate adhesive
joints
R. J. C. Carbas1,2*  , E. A. S. Marques1 and L. F. M. da Silva2

*Correspondence:
rcarbas@fe.up.pt Abstract 
1
Institute of Science The use of composite materials in structural applications has significantly expanded in
and Innovation
in Mechanical and Industrial recent years. The transport industry accounts for an increasingly larger share of the final
Engineering (INEGI), Faculty structural weight of vehicles, as manufacturers pursue improvements in fuel economy,
of Engineering, University lighter more efficient designs, and reduction of emissions. However, the delamination
of Porto, Porto, Portugal
Full list of author information of adhesively bonded composite joints causes premature failure of the bond, inhibiting
is available at the end of the the use of its full potential and leading to inefficient and over-designed components.
article A hybrid composite metallic material technology is studied in this work, a method
inspired in the fibre metal laminate concept, and which combines the best properties
of FRPs and metal alloys. The hybrid composite-metallic adherends aims to increase
the joint strength in the through thickness direction, minimise peel stresses and limit
delamination. The objective of this work was to evaluate the performance of hybrid
joints, bonded with different adhesives by comparing them against a reference joint
using a conventional Carbon fibre reinforced polymer (CFRP) adherend. The joints
were experimentally tested using a universal testing machine for a crosshead speed
of 1 mm/min. Numerical models were developed, using the ABAQUS software, to
study the behaviour of all joints studied. The numerical predictions of failure loads and
modes were compared to the experimentally obtained results.
Keywords:  Carbon fibre, Laminates, Mechanical properties, Finite element analysis,
Mechanical testing, Anodizing

Introduction
The importance of composite materials in modern engineering cannot be overstated.
Nowadays, composites represent a very important subset of materials for any designer/
engineer, mainly due to their high specific stiffness or excellent strength to weight ratio,
fatigue behaviour and corrosion resistance. This makes them very attractive for applica-
tions where weight is a major design constraint. However, joining composites is often a
challenging proposition. In most cases, the joining will be guaranteed by adhesive bond-
ing only, with adhesives taking on a critical structural role. The anisotropic nature of
composites adds an extra layer of complexity to the use of these materials with possible
out-of-plane/interlaminar loadings leading to delamination—a transversal failure mode
due to peel stresses and poor bonding between the fibres and the polymeric matrix.

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Carbas et al. Appl Adhes Sci (2021) 9:1 Page 2 of 14

Delamination is seen as a major issue to tackle before a more representative use of


composite materials in structural applications can occur, allowing to fully explore their
inherent advantages [1, 2]. Currently, there are safety concerns about the detection of
delamination cracks and, since studies show that the crack growth in CFRP is relatively
high for low stress fatigue cycles, this could lead to unpredictable catastrophic failures of
composite structures [3]. The initiation of the cracks themselves could be traced back to
geometrical discontinuities, such as the holes for mechanical fasteners or even to impact
damage [4]. In fact, the higher notch sensitivity of composites and their low shear
strength is one of the reasons that adhesive joints became prevalent over mechanical
connections for joining composites. The smooth uniform stress distribution observed
along the bond translates into excellent joint performance and high fatigue resistance.
There are several methods available to mitigate the delamination issue [5], such as
Z-pins or Z-anchoring (the introduction of thin pins, in the through thickness direction
of the composite, holding the laminate plies together by a combination of adhesion and
friction [6, 7]), 3D weaving (the reinforcement of interlaminar properties by the creation
of complex three dimensional dry fibre preforms before applying the resin [8, 9]), stitch-
ing or tufting (embedding stitch threads through thickness direction, creating a bridg-
ing effect that will attenuate the delamination cracks [10, 11]), mixed adhesive joints or
functionally graded adhesive joints (to decrease of stress concentration at the ends of
overlap and increase of joint strength using a more flexible adhesive at the ends of the
overlap to reduce the peel stresses in that critical section [12, 13]), and hybrid laminates
(metal or polymeric laminates are used to reinforce the composite transversal proper-
ties [14–17]). The 3D weaving, stitching, braiding, tufting, z-pinning and z-anchoring
techniques all successfully reduce delamination failure, but are quite laborious, which
increases the cost of the final product [18].
The use of hybrid laminate concept is a technique which is simpler to implement
industrially and can also be successful in delamination prevention. The authors showed
previously that the delamination of composite joints can be avoided by reinforcing the
composite adherends with thin metal [14–16] or polymeric layers [17]. The hybrid lami-
nate technique allows to combine the mechanical properties of different laminates rein-
forced with composite.
The aim of this study was the evaluation of the joint performance of hybrid metal lami-
nates bonded with different epoxy adhesives. The resultant hybrid joints were compared
with joints using only CFRP adherends. The joints were tested using a universal test-
ing machine at a rate speed of 1 mm/min. Numerical models were developed, using the
ABAQUS software, to better understand the behaviour of all configurations under study.
The numerical predictions of the failure loads and failure modes were compared to the
experimentally obtained results.

Experimental details
Adhesive
Three different epoxy-based adhesives were considered for this work. These are the
Araldite® AV138M with HV 998 hardener, 3M Scotch Weld AF 163 2K and Nagase
Denatite XNR6852E-3. Although they are all epoxy-based structural adhesives they
differ greatly with respect to their use and mechanical properties. The mechanical
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 3 of 14

properties of adhesives are summarized in Table 1. These properties were later used to
construct the triangular cohesive laws used for finite element modelling.

Adherends
The adherends materials for the studied joint configurations were chosen according to
their industrial relevance. The composite used was a 0° oriented carbon-epoxy compos-
ite. CFRP is an orthotropic material, whose elastic mechanical properties can be seen in
Table 2. The elastic mechanical properties of the CFRP correspond to the orientation of
a 0° CFRP ply (x—fibre, y—transverse and z—thickness directions).
The metal layers used were composed of the 2024-T3 aluminium alloy. It is a high
strength alloy and also has very good fatigue resistance. The mechanical properties of
this alloy are shown in Table 3.
The ratio of metal and CFRP in the hybrid laminate adherend was of 1:4 (25% of
metal). This ratio was selected as the proposed concept seeks the use of metal as a rein-
forcement of the CFRP, which ensures a minimal weight penalty. The hybrid laminate
used was selected based on previous studies carried out by Carbas et al. [14]. Figure 1
shows the adherend configuration of hybrid laminates where the metal layer thickness
was of 0.4 mm on each side of the CFRP core.

Specimen manufacture
As stated in the introduction, the main objective of this study was to assess the performance
of hybrid adhesive joints bonded with adhesives of different stiffness. To accomplish this
objective, single lap joints with an overlap of 50 mm, width of 25 mm and adhesive thick-
ness of 0.2 mm were manufactured. The geometry of the joints is detailed in Fig. 2.

Table 1  Mechanical properties of adhesives


AV138M1/HV998 AF 163-2K [15, Denatite
[13, 14] 17] XNR 6852
E-3 [19,
20]

Quasi-static (1 mm/min) E (MPa) 4890 1520 1728


G (MPa) 1560 565 665
σu (MPa) 39.45 46.93 51.5
τu (MPa) 30.2 46.86 44.9
GIC (N/mm) 0.346 4.05 9.2
GIIC (N/mm) 4.91 9.77 51

Table 2  Elastic properties of the CFRP [21]

Ex = 1.09E5 MPa νxy = 0.342 Gxy = 4315 MPa


Ey = 8819 MPa νxz = 0.342 Gxz = 4315 MPa
Ez = 8819 MPa νyz = 0.380 Gyz = 3200 MPa

Table 3  Mechanical properties of 2024-T3 aluminium alclad series [22]


Young’s modulus (GPa) Yield stress (MPa) Ultimate stress (MPa) Poisson’s ratio Elongation (%)

66 350 440 0.3 12


Carbas et al. Appl Adhes Sci (2021) 9:1 Page 4 of 14

Fig. 1  Adherend configuration

95 50 95 25

3.2
Adhesive thickness
of 0.2
Fig. 2  Geometry of the single lap joints (all dimensions are in mm)

Surface treatment influence


The manufacture process of the joints required careful surface preparation of the alu-
minium sheets in order to ensure a good adhesion. A previous study by Carbas et  al.
[14], found that grit blasting and degreasing with acetone was insufficient to ensure a
good level of adhesion to the aluminium laminates, resulting in a mixed cohesive-adhe-
sive failure type for the quasi-static loading condition tested. In order to evaluate the
active surface treatment that provides the best adhesion, different surface treatments
were tested. To perform this analysis, SLJs bonded with AF 163 2K were manufactured
and tested under quasi-static conditions. Different procedures were studied, with two
different methods being considered to anodise the aluminium adherend. These two
methods are phosphoric acid anodising (PAA) according to the ASTM D 3933 stand-
ard and the application of a sol–gel based anodising replacement, the 3M™ Surface Pre-
Treatment AC-130–2. Moreover, the influence of a primer (a structural adhesive primer
3M Scotch Weld EW—5000 AS) was also evaluated. Load–displacement curves high-
lighting the relative performance of the different surface treatments can be seen in Fig. 3.
The solution that provides the best bonding results for this aluminium alloy will con-
sequently be the one that produces the largest increase of the maximum displacement
before failure. This was found to be the treatment of the surface with the sol–gel Phos-
phoric Acid Anodising Replacement Solution (3M™ Surface Pre-Treatment AC-130-2),
followed by the application of the Structural Adhesive Primer EW—5000 AS. The appli-
cation of this primer was carried out by manually brushing it unto the surface.

Tensile testing
For quasi-static conditions the single lap joints were tested using an Instron 8801 servo-
hydraulic testing machine with a load cell of 100  kN at a constant crosshead speed of
1 mm/min. These tests were carried out according to ASTM D5868-01(2014) “Standard
Test Method for Lap Shear Adhesion for Fiber Reinforced Plastic Bonding” [23].
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 5 of 14

Fig. 3  Al-Adhesive-Al Surface treatment study

Fig. 4  Traction–separation law with linear softening law available in ABAQUS®

Numerical analysis
Cohesive zone models are especially well suited to simulate adhesive layers, as they com-
bine continuum mechanics (for damage initiation), and fracture mechanics (for crack
propagation). Figure 4 shows the triangular cohesive zone model (CZM) used, this law
is widely used due to its simplicity and provides good results for many applications [24].
FEM analyses were performed in the ABAQUS finite element software package
(Dassault Systèmes Simulia Corp. Providence, RI, USA) using CZM. A bi-dimensional
static analysis was used to simplify the model and reduce computational times. The ele-
ments used to mesh the model were 4-node bilinear plane strain quadrilateral elements
(CPS4R). The adhesive was modelled with 4 node cohesive elements (COH2D4). Non-
linear geometrical effects were included and the elastic orthotropic properties shown in
Table 2 were used to simulate the behaviour of the CFRP material. The boundary condi-
tions were consistent in all simulations and were as shown in Fig. 5. The left end of the
joint was fixed while in the right end a displacement was applied to replicate the loading.
The joint was also restrained transversely.
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 6 of 14

Fig. 5  Boundary conditions used

Fig. 6  a Detailed view of the 50 mm overlap joint; b enlarged detailed view in which the cohesive layers can
be observed

CFRP‑only joint
In order to allow for the simulation of the delamination process, a cohesive element
layer (0.02 mm thick) was introduced in the adherend, at a distance of 0.05 mm from the
adhesive layer. Figure 6 shows a detailed view of only-CFRP joint highlighting the loca-
tion of the cohesive layers.
This model successfully replicated the results obtained experimentally. The cohesive
zone elements placed between the layers of carbon fibre were found to become damaged
similarly to the experimental case. Two examples of the element degradation obtained
with the model are presented in Fig. 7. The stress values in the first lamina (Fig. 7a) are
very high and would lead to a fibre failure.
The traction separation law is composed of a linear elastic section, which corresponds
to a gradual loading until the stress criterion is achieved, followed by a softening phase,
which uses fracture mechanics. The latter part of the law corresponds to the damage of
the simulated material and is irreversible. In case of the law implemented in ABAQUS®,
this means that if any unloading occurs, subsequent loading will not follow the initial
path along the linear elastic region of the undamaged model, but one that terminates in
the location where the unloading occurred. The degradation of an element is a measure
of how much softening the element was subjected to.

Hybrid laminate joint


An additional model was developed in order to evaluate the behaviour of a hybrid lami-
nate joint. This laminate uses aluminium layers with a thickness of 0.4 mm (Fig. 8). As
a consequence of the high thermal stresses induced by the curing process, a two-step
analysis was used, allowing to take in consideration these pre-existing stresses.
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 7 of 14

Fig. 7  CFRP-only joint bonded with Araldite AV138; a Von Mises stress plot on the detailed view of the
delamination zone; b degradation of the cohesive zone elements

Fig. 8  AL-CFRP-AL—type laminate structure; a whole model, b detailed view

The von Mises equivalent residual thermal stresses induced due to the differences of
thermal expansion coefficient between the CFRP and Aluminium is shown in Fig. 9.
The contraction of the aluminium that will be present in the joint due the cure cycle
of the adhesive is evident.
The isotropic aluminium layer distributes the peel stress over a larger area than a
CFRP layer would do, promoting an increase of joint strength. The failure mechanism
of the hybrid laminate joints bonded with AV138 is presented in Fig. 10.
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 8 of 14

Fig. 9  Pre-existing thermal stresses (detailed view of the overlap)

Fig. 10  Detailed view of the element degradation process

Experimental results
In order to evaluate the effectiveness of the proposed hybrid laminate joint, its
mechanical performance is compared with that of joints which employ a conven-
tional only-CFRP adherend. The test specimens were bonded with different epoxy
adhesives and five specimens were manufactured for each lay-up configuration.

Araldite AV 138 joints


Figure  11 shows typical load–displacement curves for only-CFRP and hybrid lami-
nate joints bonded with Araldite AV 138.
The failure load of the CFRP-only joints showed an average failure load of
11.7 ± 0.4 kN, while for the hybrid laminate joints the failure load was 12.4 ± 0.6 kN.
The failure load increased marginally by 6.0% with the reinforcement of adherend
with aluminium sheet (the use of hybrid laminate adherends). The failure mode
for only-CFRP joints was by delamination of the adherend (Fig.  12a), while for the
hybrid laminate joints a cohesive failure in the adhesive (Fig. 12b) was encountered.
As expected, the external aluminium sheet led to an increase of the peel strength of
the adherends and allowed for an increase of load transfer, conducting to an increase
of joint strength. However, the joint strength increase is modest due to high stiffness
of the adhesive, which promoted failure close to the interface where the stresses are
higher. This observation suggests that a hybrid joint has the potential to provide a
substantial increase of joint strength should a more ductile adhesive be used.
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 9 of 14

15

12.5

10
Load [kN]

7.5

2.5
Only-CFRP joint Hybrid laminate joint

0
0 0.2 0.4 0.6 0.8 1 1.2
Displacement [mm]
Fig. 11  Typical load–displacement curves of joints bonded with Araldite AV138

Fig. 12  Failure surface of the only-CFRP joints (a) and hybrid laminate joints (b) bonded with brittle adhesive
(AV 138)

AF 163‑2K joints
Typical load–displacement curves of only-CFRP and hybrid joints bonded with 3M AF
163-2K are shown in Fig. 13.
Carbas et al. [14] studied evaluate the joint performance of only-CFRP and hybrid lam-
inate joints bonded with AF 163-2K. The failure load of the CFRP-only joints showed an
average failure load of 31.3 ± 1.9 kN, and the hybrid laminate joints failure load reached
was 39.5 ± 0.5 kN. The failure load increased by 26.2% when the adherend of adhesive
joints is reinforced with an aluminium sheet. The failure mode for CFRP only joints was
delamination (Fig. 14a), and for the hybrid laminate joints a cohesive failure in the adhe-
sive (Fig. 14b) was obtained. The decrease of stiffness and increase of toughness, when
compared the mechanical properties of AF 163-2K in relation to AV 138, allowed the
hybrid joints to obtain a cohesive failure in the middle of bondline.
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 10 of 14

Fig. 13  Typical load–displacement curves of joints bonded with AF163-2K [14]

Fig. 14  Failure surface of the only-CFRP joints (a) and hybrid laminate joints (b) bonded with AF 163-2K

XNR6852E‑3 joints
Figure  15 shows typical load–displacement curves of joints bonded with Nagase
XNR6852E-3 adhesive.
The only-CFRP joints exhibited a failure load of 35.4 ± 2.2 kN while the hybrid lami-
nate joints were found to be slightly weaker with a failure load of 32.9 ± 1.4 kN. The fail-
ure load decreased − 7.0% comparing with CFRP joints. The failure mechanism for both
joints bonded with Nagase XNR6852E-3 was cohesive failure in the adherend, more spe-
cifically delamination of the composite adherends (Fig. 16). This behaviour indicates that
the peel strength of the adhesive is higher that the peel strength of the adherend.

Discussion of joint performance


The performance of only-CFRP joints bonded with different adhesives is shown in
Fig.  17. All joints showed delamination and the adhesives with the highest toughness
showed the highest strength. The high ductility of these adhesives allows them to deform
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 11 of 14

45

40

35

30
Load [kN]

25

20

15

10

5 Only-CFRP joint Hybrid laminate joint

0
0 0.2 0.4 0.6 0.8 1 1.2
Displacement [mm]
Fig. 15  Typical load–displacement curves of joints bonded with Nagase XNR6852E-3

Fig. 16  Failure surface of only-CFRP joints (a) and hybrid laminate joints (b) bonded with Nagase
XNR6852E-3

plastically and this leads to an increase in joint performance. The existence of delamina-
tion means that is theoretically possible to obtain higher joint strength if an alternative
composite with higher peel strength is used.
Figure  18 shows the joint strength of hybrid laminate joints bonded with different
adhesives. The AF 163-2K adhesive allows the hybrid joints to reach the highest joint
strength. This indicates that both the stiffness and the strength of the adhesive should
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 12 of 14

40

35

30

Failure load [kN]


25

20

15

10

0
AV 138 AF 163-2K XNR6852E-3

Only-CFRP Numerical
Fig. 17  Failure load of only-CFRP joints bonded with different adhesives

45
40
35
Failure load [kN]

30
25
20
15
10
5
0
AV 138 AF 163-2K XNR6852E-3

Hybrid laminate Numerical


Fig. 18  Failure load of hybrid laminate joints bonded with different adhesives

noy be excessively high to attain optimal performance. In fact, the adhesive with highest
toughness (XNR6852E-3) led to a delamination failure with negative consequences on
joint strength.
A good correlation between the numerical models and the experimental results was
achieved, not only with regards to the failure load prediction, but also in respect to fail-
ure modes and load displacement curves.
The difference in joint performance between only-CFRP and hybrid laminate joints
bonded with a brittle adhesive was found to be residual at best. This is due to the stiff
nature of the adhesive, introducing a high level of stress concentration at the ends of the
overlap length. When an adhesive with high ductility and with high strength (Nagase
XNR6852E-3) is used, the failure mechanism was found to be delamination. This is due
to high peel strength of the adhesive, that promotes failure of the joints by delamina-
tion. Consequentially, the joint strength of both type of joints is the same. In contrast the
adhesive with intermediate strength and with higher ductility is the adhesive that allows
Carbas et al. Appl Adhes Sci (2021) 9:1 Page 13 of 14

to attain the largest performance improvement. This adhesive provides an effective path
for load transfer through all the bonded area.

Conclusion
The main objective of this work was understanding if the strength of composite joints
could be increased with the use of hybrid laminate adherends. In order to accomplish
this goal, experimental and numerical procedures were carried out, considering differ-
ent epoxy adhesives in order to better understand how adhesive properties influence the
strength of hybrid adhesive joints. The experimental tests and numerical simulations
allowed to precisely evaluate the strength and the failure mechanisms of the designed
joints. This study showed that sol–gel and primer was the best surface treatment to use
in order ensure a good adhesion.
Different epoxy adhesives were used, and it was demonstrated that the performance of
hybrid laminate joint was heavily dependent on the mechanical properties of the adhe-
sives used. The AF163-2K adhesive was found to behave better than stronger and stiffer
adhesives in delamination prevention.
The numerical models developed in ABAQUS® showed a good agreement with the
joint strength obtained experimentally. The thermal stresses analysis proved that high
residual thermal stresses are present in the hybrid laminate joint, due to the very low
thermal expansion coefficient of CFRP. The average equivalent von Mises stress is nor-
mally, in this setup, higher than half of the yield strength of the aluminium alloy.

Abbreviations
CFRP: Carbon fibre reinforced polymer; 3D: Tri-dimensional; E: Young’s modulus; ν: Poisson’s ratio; G: Shear modulus; PAA:
Phosphoric acid anodising; CZM: Cohesive zone model.

Acknowledgements
R. J. C. Carbas would like to thank the Portuguese Foundation for Science and Technology (FCT) for supporting the work
presented here, through the individual grant SFRH/BPD/96992/2013.

Authors’ contributions
RJCC—This researcher carried out the experimental tests and write this part in the manuscript. EASM—This researcher
carried out the numerical study and write this part in the manuscript. LFMdS—This researcher was the mentor of this
concept of hybrid joints, he reviewed all the manuscript. All authors read and approved the final manuscript.
Funding
This research was funded by Portuguese Foundation for Science and Technology (FCT) under individual grant SFRH/
BPD/96992/2013.

Availability of data and materials


All relevant data is presented in the manuscript and additional information can be made available on request if
necessary.

Competing interests
The authors declare that they do not have competing interests.

Author details
1
 Institute of Science and Innovation in Mechanical and Industrial Engineering (INEGI), Faculty of Engineering, University
of Porto, Porto, Portugal. 2 Department of Mechanical Engineering, Faculty of Engineering, University of Porto, Porto,
Portugal.

Received: 26 November 2020 Accepted: 18 December 2020

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